Engineering interfacial adhesion for high-performance lithium metal anode

Suppressing lithium dendrites in carbonate electrolyte remains a grand challenge for high voltage lithium metal batteries. The role of adhesion between the interfacial layer and the lithium metal in controlling lithium growth is often overlooked. Here, we find that the adhesion energy significantly influences lithium dendrite growth by the phase-field simulations, and LiAl is an attractive material with strong adhesion with lithium metal by density functional theory (DFT) calculations. Then a simple solution process is developed to form conformal nanostructured LiAl interfacial layer on the lithium metal surface. With the nanostructured LiAl alloy-based interfacial layer, the Li/Li symmetric cell can be cycled stably for more than 1100 times at 5 mA/cm², 1 mAh/cm² with a low overpotential of 170 mV. For the LiNi_1/3Co_1/3Mn_1/3O₂/Li full cell, this interfacial layer improves the capacity retention from 59.8% to 88.7% for 120 cycles at 1 C rate, and for the LiFePO₄/Li system, the modified lithium anode also improves capacity retention from 79.5% to 99.4% after 150 cycles. This study represents a new approach to enhance the performance of lithium anode for rechargeable batteries with high voltage and high energy density.